"Nanoscience is a hot issue right now, and people are trying to create self-assembled
nanoparticle arrays for data and memory storage," Argonne assistant physicist
Zhang Jiang said. "In these devices, the degree of ordering is an important
factor."

Assistant physicist Zhang Jiang (from left) examines a X-ray diffraction as physicist Jin Wang and nanoscientist Xiao-Min Lin prepare a sample at one of the Advanced Photon Source’s beamlines. The Argonne scientists have examined nanoparticle crystallization in unprecedented detail using the high powered X-rays of the APS.

In order to call up a specific bit of data, it is ideal to store information
on a two-dimensional crystal lattice with well-defined graphical coordinates.
For example, every bit of information of a song saved on a hard drive must be
stored at specific locations, so it can be retrieved later. However, in most
cases, defects are inherent in nanoparticle crystal lattices.

"Defects in a lattice are like potholes on a road," Argonne physicist
Jin Wang said. "When you're driving on the highway, you would like
to know whether it is going to be a smooth ride or if you will have to zigzag
in order to avoid a flat tire. Also, you want to know how the potholes form
in the first place, so we can eliminate them."

Controlling the degree of ordering in nanoparticle arrays has been elusive.
The number of nanoparticles a chemist can make in a small volume is astonishingly
large.

"We can routinely produce 1014 particles in a few droplets of solution.
That is more than the number of stars in the Milky Way Galaxy," Argonne
nanoscientist Xiao-Min Lin. "To find conditions under which nanoparticles
can self-assemble into a crystal lattice with a low number of defects is quite
challenging."

Because nanoparticles are so small, it is not easy to see how ordered the lattice
is during the self-assembly process. Electron microscopy can see individual
nanoparticles, but the field of view is too small for scientists to get a "big
picture" of what the ordering is like in macroscopic length scale. It
also doesn't work for wet solutions.

"With local ordering, one cannot assume the same order exists throughout
the whole structure; it's like seeing a section of road and assuming it
is straight and well constructed all the way to the end," Wang said.

The same group of researchers at Argonne, together with their collaborators
at the University of Chicago, discovered that under the right conditions, nanoparticles
can float at a liquid-air interface of a drying liquid droplet and become self-organized.

This allows the two-dimensional crystallization process to occur over a much
longer time scale. "You typically don't expect metallic particles
to float. It is like throwing stones into a pond and expecting them to float
on the surface," Lin said. "But in the nanoworld, things behave
differently."

Using high-resolution X-ray scattering at the Advanced Photon Source (APS),
Jiang and the others examined the crystallization process in unprecedented detail
as it forms in real time. They discovered that the nanoparticle arrays formed
at the liquid-air interface can enter a regime of a highly crystalline phase
defined in the classical two-dimensional crystal theory. Only when the solvent
starts to dewet from the surface, do defects and disorder begin to appear.

"We can probe the entire macroscopic sample and monitor what's
happening in real time," Jiang said. "This allows us to understand
what parameters are important to control the self-assembly process."

With this level of understanding, the scientists hope that one day devices
such as the iPod Nano can be made from nanoparticles.

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